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Magnetic Magnetoelectric and Magnetoelastic Properties of new multiferroic material NdFe3(BO3)4

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 Publication date 2006
  fields Physics
and research's language is English




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Complex experimental and theoretical study of the magnetic, magnetoelectric, and magnetoelastic properties of neodymium iron borate NdFe3(BO3)4 along various crystallographic directions have been carried out in strong pulsed magnetic fields up to 230 kOe in a temperature range of 4.2-50 K. It has been found that neodymium iron borate, as well as gadolinium iron borate, is a multiferroic. It has much larger (above 3 10^(-4) C/m^2) electric polarization controlled by the magnetic field and giant quadratic magnetoelectric effect. The exchange field between the rare-earth and iron subsystems (~50 kOe) has been determined for the first time from experimental data. The theoretical analysis based on the magnetic symmetry and quantum properties of the Nd ion in the crystal provides an explanation of an unusual behavior of the magnetoelectric and magnetoelastic properties of neodymium iron borate in strong magnetic fields and correlation observed between them.



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We report the low-temperature coexistence in NdFe3(BO3)4 of an incommensurate magnetic phase with a strained commensurate magnetic phase that is primarily at the surface of the crystal. Increasing the temperature or magnetic field decreases the incommensurability and stabilizes the commensurate magnetic phase above Tic ~14 K or Hic = 0.9 T. A comparison to published studies indicates the onset of longitudinal magnetostriction and electric polarization at the magnetic-field-induced transition, which may arise due to a basal plane spin-flop and canting of the moments along the field direction.
We report high-resolution optical absorption spectra for NdFe3(BO3)4 trigonal single crystal which is known to exhibit a giant magnetoelectric effect below the temperature of magnetic ordering TN = 33 K. The analysis of the temperature-dependent polarized spectra reveals the energies and, in some cases, symmetries and exchange splittings of Nd3+ 84 Kramers doublets. We perform crystal-field calculations starting from the exchange-charge model, obtain a set of six real crystal-field parameters, and calculate wave functions and magnetic g-factors. In particular, the values g(perpendicular) = 2.385, g(parallel) = 1.376 were found for the Nd3+ ground-state doublet. We obtain Bloc=7.88 T and |JFN|= 0.48 K for the values of the local effective magnetic field at liquid helium temperatures at the Nd3+ site and the Nd - Fe exchange integral, respectively, using the experimentally measured Nd3+ ground-state splitting of 8.8 cm-1. To check reliability of our set of crystal field parameters we model the magnetic susceptibility data from literature. A dimer containing two nearest-neighbor iron ions in the spiral chain is considered to partly account for quasi-one-dimensional properties of iron borates, and then the mean-field approximation is used. The results of calculations with the exchange parameters for Fe3+ ions Jnn = -6.25 K (intra-chain interactions) and Jnnn = -1.92 K (inter-chain interactions) obtained from fitting agree well with the experimental data.
Nowdays, multiferroic materials with magnetoelectric coupling have many real-world applications in the fields of novel memory devices. It is challenging is to create multiferroic materials with strongly coupled ferroelectric and ferrimagnetic orderings at room temperature. The single crystal of ferric selenide (Fe3Se4) shows type-II multiferroic due to the coexistence of ferroelectric as well as magnetic ordering at room temperature. We have investigated the lattice instability, electronic structure, ferroelectric, ferrimagnetic ordering and transport properties of ferroelectric metal Fe3Se4. The density of states shows considerable hybridization of Fe-3d and Se-4p states near the Fermi level confirming its metallic behavior. The magnetic moments of Fe cations follow a type-II ferrimagnetic and ferroelectric ordering with a calculated total magnetic moment of 4.25 per unit cell (Fe6Se8). The strong covalent bonding nature of Fe-Se leads to its ferroelectric properties. In addition, the symmetry analysis suggests that tilting of Fe sub-lattice with 3d-t2g orbital ordering is due to the Jahn-Teller (JT) distortion. This study provides further insight in the development of spintronics related technology using multiferroic materials.
Comprehensive studies of magnetic properties of GdCr3(BO3)4 single crystal have been carried out. The integrals of intrachain and interchain exchange interactions in the chromium subsystem have been determined and the strength of Cr-Gd exchange interaction has been estimated. The values of the exchange field and the effective magnetic anisotropy field of GdCr3(BO3)4 have been estimated. The electric polarization along the a axis in the longitudinal geometry of the experiment has been detected. Correlations between the electric polarization and the magnetization of the studied compound have been found. The spin-reorientation phase transition in the magnetically ordered state has been found. This transition exists for the external magnetic field applied along any crystallographic direction and the transition field depends weakly on the direction of the field. The nature of the spin-reorientation phase transition has been discussed. Magnetic phase diagram has been constructed and spin configurations for the low-field and high-field phases have been proposed.
Clear anomalies in the lattice thermal expansion (deviation from linear variation) and elastic properties (softening of the sound velocity) at the antiferromagnetic-to-paramagnetic transition are observed in the prototypical multiferroic BiFeO3 using a combination of picosecond acoustic pump-probe and high-temperature X-ray diffraction experiments. Similar anomalies are also evidenced using first-principles calculations supporting our experimental findings. Those calculations in addition to a simple Landau-like model we also developed allow to understand the elastic softening and lattice change at T_N as a result of magnetostriction combined with electrostrictive and magnetoelectric couplings which renormalize the elastic constants of the high-temperature reference phase when the critical T_N temperature is reached.
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